standard of electrolysis, such criteria are critical and still challenging. For energy storage devices, such as supercapacitors, an active catalyst capable of providing high power density and superior cycle life is a necessary condition. Pseudo capacitors exhibit very high-power density similar to that of double-layer capacitor devices. However, they differ from a double-layer capacitor because of their battery-like redox processes of the charge storage principles. Transition metal oxides (TMOs) such as NiCo 2 O 4 @NiMoO 4 , [6] NiCo-S (Fe-NiCo-S), [7] CoMxP/CC (M = Fe, Mn, and Ni), [8] and NiCoFe-P [9] have been employed as active electrocatalysts for OER and supercapacitors. Pseudocapacitive-type nanomaterials, especially TMOs or hydroxides, such as nickel oxide (NiO), [10,11] NiMoO 4 @Co (OH) 2 , [12] are widely investigated as candidates for supercapacitor applications due to their various oxidation states that contribute to the pseudo capacitance properties.Hierarchical-structured catalysts have attracted considerable attention in the field of materials for renewable energy applications. These structures can effectively increase the active surface area owing to their morphology. We recently reported the catalytic efficiency of hydrated core NiMoO 4 and shell Co 3 O 4 Hierarchical nanostructures have attracted considerable research attention due to their applications in the catalysis field. Herein, we design a versatile hierarchical nanostructure composed of NiMoO 4 nanorods surrounded by active MoS 2 nanosheets on an interconnected nickel foam substrate. The as-prepared nanostructure exhibits excellent oxygen evolution reaction performance, producing a current density of 10 mA cm −2 at an overpotential of 90 mV, in comparison with 220 mV necessary to reach a similar current density for NiMoO 4 . This behavior originates from the structural/morphological properties of the MoS 2 nanosheets, which present numerous surface-active sites and allow good contact with the electrolyte. Besides, the structures can effectively store charges, due to their unique branched network providing accessible active surface area, which facilitates intermediates adsorptions. Particularly, NiMoO 4 /MoS 2 shows a charge capacity of 358 mAhg −1 at a current of 0.5 A g −1 (230 mAhg −1 for NiMoO 4 ), thus suggesting promising applications for charge-storing devices.